The crystalline structure, magnetism, and magnetocaloric effect of a GdCrO3 single crystal grown with the laser-diode-heated floating-zone technique have been studied. The GdCrO3 single crystal crystallizes into an orthorhombic structure with the space group P mnb at room temperature. Upon cooling, under a magnetic field of 0.1 T, it undergoes a magnetic phase transition at TN-Cr = 169.28(2) K with Cr 3+ ions forming a canted antiferromagnetic (AFM) structure, accompanied by a weak ferromagnetism. Subsequently, a spin reorientation takes place at TSR = 5.18(2) K due to Gd 3+ -Cr 3+ magnetic couplings. Finally, the long-range AFM order of Gd 3+ ions establishes at T N-Gd = 2.10(2) K. Taking into account the temperature-(in)dependent components of Cr 3+ moments, we obtained an ideal model in describing the paramagnetic behavior of Gd 3+ ions within 30-140 K. We observed a magnetic reversal (positive → negative → positive) at 50 Oe with a minimum centering around 162 K. In the studied temperature range of 1.8-300 K, there exists a strong competition between magnetic susceptibilities of Gd 3+ and Cr 3+ ions, leading to puzzling magnetic phenomena. We have built the magnetic-field-dependent phase diagrams of T N-Gd , TSR, and TN-Cr, shedding light on the nature of the intriguing magnetism. Moreover, we calculated the magnetic entropy change and obtained a maximum value at 6 K and ∆µ0H = 14 T, i.e., -∆SM ≈ 57.5 J/kg.K. Among all RECrO3 (RE = 4f n rare earths, n = 7-14) compounds, the single-crystal GdCrO3 compound exhibits the highest magnetic entropy change, as well as an enhanced adiabatic temperature, casting a prominent magnetocaloric effect for potential application in magnetic refrigeration.