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Abstract Manipulating the stoichiometric distribution along depth direction is a promising technique to modulate the optical and optoelectronic properties of the mid-infrared sensitive lead chalcogenides at room temperature. Here, we demonstrate an optoelectronic sensitization method based on O+ beam implantation at 50 kV for polycrystalline PbSe, which can manipulate the depth profile and hence the structural properties to modulate the optical and the optoelectronic performances. Unlike the diffused material presented in previous works, the resulting material is nano-polycrystalline with average grain sizes of 17.1–29.3 nm. The optoelectronic characterizations indicate that the optoelectronic properties can indeed be modulated by the implantation dose. The responsivity up to 2.09 A/W at 4 μm has been obtained at room temperature from the sample with implantation dose of 1 × 1018 cm−2. Comparing with the diffusion counterpart, the ion prepared PbSe nanomaterial exhibits completely different structural, compositional, optical, and electrical properties. The high responsivity of this material is attributed to the high optical absorption and carrier mobility induced by O+ beam. However, the high dark current has been also observed in this material, mainly due to its low inherent potential barrier height between crystallites. Graphical abstract Image 1 Highlights • An ion beam technology for preparing mid-infrared photosensitive PbSe nanomaterial has been presented. • Enhanced optical absorption, carrier mobility and photo-responsivity have been induced by this technology. • The low potential barrier height between crystallites of this nanomaterial is caused by its small particle sizes. • The microstructure and the optoelectronic properties can be modulated by the implantation dose. [ABSTRACT FROM AUTHOR]