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Combining functional metal nanoparticles with materials from other families may lead to nanocomposites with enhanced properties and unique multi-functionalities suitable for a wide range of applications. In this work, direct current atmospheric pressure microplasma (or microplasma) has been deployed for the synthesis of functional gold nanoparticle/nanocarbon nanocomposites and silver nanoparticle/polymer nanocomposites for the first time. Different experimental parameters, such as precursor concentration, solution pH, plasma processing time, etc., have been investigated to understand their effects on the resulting nanocomposite structures and properties. The nanocomposites were fully characterized using a wide range of materials characterization techniques. Potential reaction pathways within the microplasma– liquid system as well as the formation mechanisms of each composite system have been proposed. Finally, the potential of these nanocomposites towards specific applications, such as surface enhanced Raman scattering sensing, photothermal conversion or antibacterial application, has been demonstrated. The results show that microplasma–liquid interaction is a “greener”, rapid and versatile technique which can be deployed for the synthesis of a wide range of functional nanocomposites. By manipulating the test parameters, one can tune the nanocomposites structures and hence optimize their properties and functionality towards specific applications. Through this work, a more in-depth understanding of the multi-phase system (consisting of gas, plasma, liquid and solid) has been established, such understanding may shine a light on the future design and fabrication of new functional nanocomposites deploying microplasma.