Biochar-based fertilizers have attracted increased attention, because biochar can improve the soil fertility, promote plant growth and crop yield. However, biochar-based controlled release nitrogen fertilizers (BCRNFs) still face problems because of the high cost, inefficient production technology, instability of nitrides, and the challenge associated with the controlled release of nutrients. In this study, we hydrothermally synthesised novel BCRNFs using urea-loaded biochar, bentonite and polyvinyl alcohol for controlled release of nutrients. Scanning electron microscopy and gas adsorption were conducted to identify the urea-loading and storage of bentonite in the inner pores of the biochar particles. X-ray diffraction, Fourier transform infrared spectroscopic and X-ray photoelectron spectroscopic studies demonstrated that strengthening the interactions among biochar, urea, and bentonite, helps control the moisture diffusion and penetration of bentonite, thereby leading to nutrient retention. The BCRNF showed significantly improved nutrient release characteristic compared with that of a mixture of biochar and urea. This urea-bentonite composite loaded with urea provides control over the release of nutrients stored in the biochar. BCRNF, especially those produced hydrothermally, can have potential applications in sustainable food security and green agriculture.