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Designing and synthesizing highly efficient hydrogen-producing catalysts using morphological control techniques and path structure layouts based on photogenerated electron migration can effectively address environmental pollution and promote clean energy development. However, exploitating stabilized photocatalysts with exceptional photocatalytic performance remains challenging. Herein, Ni3S4/ZnCdS quantum dots (NZCS QDs) were synthesized at room temperature for high-efficiency photocatalytic H2 production. l-Cysteine (l-Cys) as constitution controller controlled the composition of the NZCS QDs by limiting their growth, and the photogenerated electrons of the cocatalyst Ni3S4 rapidly captured the photogenerated holes of ZCS QDs. This process resulted in a significant increase in the H2 evolution rate of NZCS QDs up to 5.03 mmol·g–1·h–1, which was 8.98 times greater than that of CdS QDs. The experimental findings indicated that the increased rate of H2 production was primarily attributed to the higher number of active sites, faster type-S photogenerated electron–hole separation driven by an internal electric field, and enhanced charge reaction efficiency of the NZCS QDs. This study presents a credible synthetic approach for NZCS QDs and offers a solution to improve the efficiency of photocatalytic reactions based on ZnCdS. [ABSTRACT FROM AUTHOR]