Magnetic refrigeration based on the magnetocaloric effect (MCE) is an environment-friendly, high-efficiency technology. It has been believed that a large MCE can be realized in the materials with a first-order magnetic transition (FOMT). Here, we found that TlFe3Te3 is a ferromagnetic metal with a first-order magnetic transition occurring at Curie temperature TC = 220 K. The maximum values of magnetic entropy change (Δ) along the crystallographic c-axis, estimated from the magnetization data, reach to 5.9 J kg−1K−1 and 7.0 J kg−1 K−1 for the magnetic field changes, ΔH = 0–1 T and 0–2 T, respectively, which is significantly larger than that of MCE materials with a second-order magnetic transition (SOMT). Besides the large ΔSM, the low-level both thermal and field hysteresis make TlFe3Te3 compound an attractive candidate for magnetic refrigeration. Our findings should inspire the exploration of high performance new MCE materials.