Experimental investigations of the magnetocaloric response of the intermetallic layered AlFe2B2 compound along the principle axes of the orthorhombic cell were carried out using aligned plate-like crystallites with an anisotropic [101] growth habit. Results were confirmed to be consistent with density functional theory calculations. Field-dependent magnetization data confirm that the a-axis is the easy direction of magnetization within the (ac) plane. The magnetocrystalline anisotropy energy required to rotate the spin quantization vector from the c-to the a-axis direction is determined as K~0.9 MJ/m3 at 50 K. Magnetic entropy change curves measured near the Curie transition temperature of 285 K reveal a large rotating magnetic entropy change of 1.3 J*kg-1K-1 at μ0Happ=2 T, consistent with large differences in magnetic entropy change ΔSmag measured along the a-and c-axes. Overall, this study provides insight of both fundamental and applied relevance concerning pathways for maximizing the magnetocaloric potential of AlFe2B2 for thermal management applications.