A structured least squares (SLS)-based ESPRIT algorithm for direction-of-arrival (DOA) estimation of strictly second-order noncircular signals using a crossed array is devised in this paper. Unlike the conventional ESPRIT for noncircular signals, which employs the least squares or total least squares, the proposed solution is able to exploit the overlapping structure of the subarray configurations to efficiently solve the shift-invariant equations (SIEs), ending up with the SLS solution for a three-axis crossed array. Moreover, an additional constraint requiring the SIEs of the three linear subarrays directed along the x-, y-, and z-axes to share the same set of eigenvectors is applied to solve the rank-deficiency problem. Consequently, the proposed approach provides more accurate DOA estimates, and its superiority over existing ESPRIT schemes is demonstrated via computer simulations.