Magnetic anisotropy is a pivotal parameter that determines the magnetic ordering behavior and plays an important role in practical applications of magnetic materials. However, its influence on thermodynamic properties remains experimentally unexplored. As an air-stable, antiferromagnetic (AFM) van der Waals (vdW) semiconductor, CrSBr exhibits unique uniaxial in-plane magnetic anisotropy, making it an ideal platform to elucidate these unresolved relationships. Herein, high-quality CrSBr single crystals are synthesized via a modified two-step chemical vapor transport (CVT) method. A comprehensive analysis using modified Arrott plots, the Kouvel-Fisher method, the Widom scaling law, and critical isotherm analysis confirms a possible direct crossover from the tricritical mean-field behavior to the 3D Ising behavior, suggesting non-negligible interlayer coupling in bulk CrSBr. Supported by first-principles calculations and molecular field approximations, a pronounced triaxial magnetic anisotropy is quantified, with relative anisotropy energy satisfying $K\left(b\to c\right)>K\left(b\to a\right)$. Notably, strong anisotropy energy overcomes the interlayer exchange coupling $\left(K>J{S}^2\right)$, driving a field-induced first-order spin-flip transition along the easy $b$ axis. The maximum magnetic entropy change ($-\mathrm{\Delta }{S}_{\mathrm{M}}^{\max }$) is 5.21, 5.09 and 4.74 J/(kg K) for $H\parallel b$, $H\parallel a$, and $H\parallel c$, respectively. Pronounced in-plane uniaxial magnetic anisotropy guarantees an anisotropic magnetocaloric effect, as evidenced by a negative linear correlation between $K$ and rotating magnetic entropy change $-\mathrm{\Delta }{S}_{\mathrm{M}}^{\mathrm{R}}$. These findings contribute to understanding of magnetism and associated thermodynamic properties in triaxially magnetically anisotropic CrSBr, thereby facilitating the tuning of magnetic anisotropy and exotic spin states in two-dimensional magnets.

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• Magnetic anisotropy
• Magnetism
• Antiferromagnets
• Semiconductor compounds
• van der Waals systems
• Density functional calculations
• Magnetization measurements