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Vacancy regulation is considered to be an effective means to improve the properties of materials, which has been applied in the fields of catalysis, electricity and optics. Herein, different contents of nitrogen vacancy in graphitic carbon nitride (g-C 3 N 4) could be modulated via changing temperature of secondary calcination. Results showed the introduction of nitrogen vacancy significantly promoted the cataluminescence (CTL) intensity towards ammonium sulfide ((NH 4) 2 S) and the CTL performance increased regularly with the increaseing vacancy content. The positive effect of nitrogen vacancy on CTL intensity of (NH 4) 2 S was unveiled in-depth by the experiment and density functional theory (DFT). Moreover, a cutting-edge CN-600-based sensor was established for the highly sensitive detection of (NH 4) 2 S. The sensor possessed excellent selectivity and stability, and a low detection limit (0.16 μg mL−1). Noteworthily, this study presents novel mentality for designing materials with improved catalytic activity. [Display omitted] • The nitrogen vacancy content in g-C 3 N 4 was successfully modulated by adjusting temperature of secondary calcination. • The mechanism of enhanced CTL performance of (NH 4) 2 S on g-C 3 N 4 surface modulated by nitrogen vacancy was revealed. • The constructed CN-600-based sensor exhibited excellent selectivity and stability for (NH 4) 2 S sensing. [ABSTRACT FROM AUTHOR]