The formation of chemical bonds between metal ions and their supports is an effective strategy to achieve good catalytic activity. However, both the synthesis of active metal species on a support and control of their coordination environment are still challenging. Here, we show the use of an organic compound to produce tubular carbon nitride (TCN) as a support for Pd nanoparticles (NPs), creating a composite material (NP-Pd-TCN). It was found that Pd ions preferentially bind with the electron-rich N atoms of TCN, leading to strong metal–support interactions that benefit charge transfer from g-C₃N₄ to Pd. X-ray absorption spectroscopy further revealed that the metal–support interactions resulted in the formation of Pd–N bonds, which are responsible for the improvement in the charge dynamics as evidenced by the results from various techniques including photoluminescence (PL) spectroscopy, photocurrent measurements, and electrochemical impedance spectroscopy (EIS). Owing to the good dynamical properties, NP-Pd-TCN was used for photocatalytic hydrogen evolution under visible-light irradiation (λ > 420 nm) and an excellent evolution rate of ~ 381 μmol·h ⁻¹ (0.02 g of the photocatalyst) was attained. This work aims to promote a strategy to synthesize efficient photocatalysts for hydrogen production by controllably introducing metal nanoparticles on a support and in the meantime forming chemical bonds to achieve intimate metal-support contact.