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Recently, the inherent piezoelectric properties of the 2D transition-metal dichalcogenides (TMDs) tin monosulfide (SnS) and tin disulfide (SnS 2 ) have attracted much attention. Thus the piezoelectricity of these materials has been theoretically and experimentally investigated for energy-harvesting devices. However, the piezoelectric output performance of the SnS 2 - or SnS-based 2D thin film piezoelectric nanogenerator (PENG) is still relatively low, and the fabrication process is not suitable for practical applications. Here we report the formation of the SnS 2 /SnS heterostructure thin film for the enhanced output performance of a PENG using atomic layer deposition (ALD). The piezoelectric response of the heterostructure thin film was increased by ∼40% compared with that of the SnS 2 thin film, attributed to large band offset induced by the heterojunction formation. Consequently, the output voltage and current density of the heterostructure PENG were 60 mV and 11.4 nA/cm 2 at 0.6% tensile strain, respectively. In addition, thickness-controllable large-area uniform thin-film deposition via ALD ensures that the reproducible output performance is achieved and that the output density can be lithographically adjusted depending on the applications. Therefore, the SnS 2 /SnS heterostructure PENG fabricated in this work can be employed to develop a flexible energy-harvesting device or an attachable self-powered sensor for monitoring pulse and human body movement.