We have studied the magnetocaloric effect (MCE) in a bilayered La4/3Sr5/3Mn2O7 single crystal with applied field along both ab-plane and c-direction. Due to the quasi-two-dimensional structure, the crystal exhibits a strong anisotropy in the MCE. The difference of magnetic entropy change between two crystallographic directions depends on external magnetic fields and has a maximum of 2J/kgK. A large low-field magnetic entropy change, reaching 3.2J/kgK for a magnetic field change of 15kOe, is observed when the applied field is along ab-plane. This large low-field magnetic entropy change is attributed to the rapid change of magnetization in response to external magnetic fields in the easy magnetizing plane.