Nowadays, many high-field magnets take advantage of the superior properties of superconductors. The superconducting square coil, a promising alternative for building Helmholtz coil has aroused great interest. This paper focuses on the critical current angular dependence of a superconducting square coil. The critical current of the entire coil and two selected strands under different magnitudes and orientations of external magnetic fields have been measured. The critical regions of the coil in different angular regimes were determined. A better understanding of the in-field performance of superconducting square coil is obtained.