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Levels of tobacco smoking among looked-after children (LAC) substantially exceed those reported among the general youth population. Research highlights that smoking is common among LAC, further increasing the health and social inequality experienced by this vulnerable group. However, there is limited research evidence about smoking and the factors that influence tobacco use in residential units, and if opportunities exist to address tobacco use in residential care. The overall purpose of this thesis was to develop a theory- and evidence-based intervention to address tobacco use in residential units for LAC. This thesis adopted both quantitative and qualitative methods in a pragmatic mixed-methods design, and followed the developmental phase of the United Kingdom Medical Research Council framework for the development and evaluation of complex interventions. It comprised three stages. The first stage comprised a review of published articles describing interventions that aimed to address the lifestyle behaviours of residentially accommodated LAC. The purpose of the review was to assess the status of the literature, identify existing effective interventions, and to explore implementation issues in residential settings. Four articles describing two interventions targeting lifestyle behaviours among residentially accommodated LAC were identified. None of the articles specifically targeted tobacco use. However, descriptions of the implementation issues likely to be encountered were provided. To complement the existing evidence, two primary research studies were conducted. First, a quantitative retrospective case-note evaluation of statutory health assessment documentation (n=31) was carried out to assess prevalence and characteristics of residentially accommodated LAC, including those who smoke and to identify current smoking-related practice. According to statutory health assessment documentation enquiries about smoking were made in 23 (77%) instances. Twelve (52%) of those children who had participated in the health assessment and who received enquiries about smoking were identified as smokers. Smoking was found to be significantly more common among LAC over the age of 15 years [p=0.043, OR3.33, (95%CI 0.91-12.27)] and more frequently reported among LAC with mental health disorder (58%). Nine (75%) smokers were recorded as engaging in discussions about their smoking and as being offered treatment for tobacco dependence. Just two of the nine (22%) smokers accepted a referral for treatment. Second, a sequential, mixed-methods study comprising a cross-sectional survey of Residential Care Officers (RCOs) in the East Midlands (n=42) and semi-structured interviews with RCOs and residential unit managers (n=14) to explore and understand the use of tobacco in residential units, from the perspective of residential carers. Survey data were analysed descriptively and findings informed the development of a schedule of topics for discussion during the subsequent interviews. Qualitative data were analysed using a thematic framework approach. Forty-two RCOs (18% response rate) completed the survey, and 14 participants took part in the interviews. Despite reporting substantial awareness of smoke-free policies, a lack of adherence and enforcement became apparent, and levels of reported training in relation to smoking and smoking cessation were low (21%). Potential problems relating to wider tobacco-related harms, such as exploitative relationships; a reliance on tacit knowledge; and pessimistic attitudes towards LAC quitting smoking, were reported. Stage two synthesised the findings from the case-note evaluation and the mixed-methods study using an existing socioecological model, to identify 33 factors as influencing tobacco use in residential units for LAC, across seven interacting levels. A consultation with four local authority and community health stakeholders identified behaviours to target with an intervention and explored challenges and enablers to implementation. Strategies that address the wider harms of tobacco use by LAC, facilitate the implementation of completely smoke-free residential units, and those which encourage and support smoking cessation among LAC were prioritised by stakeholders, achieving mean scores of 4.5 (SD 0.57), 3.25 (SD 1.25), and 3.0 (SD 1.41) from a maximum of five points, respectively. Stakeholders identified 16 barriers and five facilitators to behavioural change and 13 implementation issues. Nine behaviours were identified as being amenable to change. In stage three, an exercise to develop potential intervention components involved mapping behavioural change targets and implementation issues to the Theoretical Domains Framework and the Diffusion of Innovation in Service Organisations model in order to identify and select behavioural change techniques and mode of intervention component delivery using the behavioural change technique taxonomy. Seven behavioural change techniques and ten modes of intervention delivery were selected from the behavioural change technique taxonomy to address target behaviours. The behavioural change techniques and modes of delivery were then modelled into an intervention comprising five components (stakeholder meeting, local leader engagement, a tobacco training programme, a smoke-free co-ordinator, and resources and tools). Finally, two social care professionals reviewed the intervention components and confirmed its relevance and utility to residential carers and their practice. In conclusion, the studies undertaken in this thesis have widened the understanding of tobacco use among LAC and has led to the development of a potential intervention to address this concern. While the intervention requires refinement and piloting before effectiveness can be determined, nonetheless, this thesis has addressed calls from successive governments, third-sector organisations, and health and social care professionals to examine and address the health needs of LAC. It is hoped that this research will lead to better awareness of the risks of smoking among LAC, and ultimately improve the health and social outcomes of LAC. Recommendations for further research are also made.