To obtain optimal luminescence, 0.12 g of GdVO4:3%Eu3+ nanocrystals (NCs) and different volumes of nitrogen‐doped carbon dots (N‐CDs) crude solution were used as precursors, and the composite synthesized using the hydrothermal deposition method showed optimal luminescence when 11 ml (2.45 mmol) crude solution was used. In addition, similar composites with the same molar ratio as GVE/cCDs(11) were also prepared with the hydrothermal and physical mixing processes. Based on the test results of XRD, XPS, and PL spectra, for the composite GVE/cCDs(11), the highest (lowest) peak intensity of the C–C/C=C (C=O/C=N) bond, which was 1.18 (0.75) times that of GVE/cCDs‐m, indicated most N‐CDs deposition and led to their highest emission intensity under 365 nm excitation, although nitrogen atoms in the composite were shed slightly during the deposition process. Finally, as can be seen from the patterns designed for security applications that the optimally luminescent composite is one of the most promising candidates in the anti‐counterfeiting field.