The main subject of this research is the development of a suitable, efficient, and biocompatible carbon nanofiber-based catalytic system for the synthesis of coumarin and 1,2,4,5-tetra-substituted imidazoles. Brønsted acid carbon nanofiber/taurine catalyst was made during three steps: acid treatment, acylation, and then amination. The basic principles and general advantages of the synthesis method are elaborated. The acidity of the prepared nano-catalyst was investigated using the Hammet acidity technique and UV–Vis spectroscopy, and the H0 value for 5 × 10–2 mg/mL of CNF/T in 0.3 mM 4-nitroaniline solution was determined to be 1.47. The structure of the catalyst was successfully characterized using FT-IR, TGA, FESEM, XRD, TEM, EDX, EDS-MAP, BET, and XPS techniques. Here, we report the ability of carbon nanofiber/taurine as a Brønsted acid catalyst for the synthesis of coumarins and 1,2,4,5-tetra-substituted imidazole through a metal-free, cost-effective, and biocompatible multicomponent route. Among the advantages of this protocol are reaction time, excellent efficiency, reusability, and high activity of the catalyst.