In this paper, the direction of arrival (DOA) estimation problem for the unfolded coprime linear array (UCLA) is researched. Existing common stacking subarray-based methods for the coprime array are invalid in the case of its subarrays, which have the same steering vectors of source angles. To solve the phase ambiguity problem, we reconstruct an improved unfolded coprime linear array (IUCLA) by rearranging the reference element of the prototype UCLA. Specifically, we design the multiple coprime inter pairs by introducing the third coprime integer, which can be pairwise with the other two integers. Then, the phase ambiguity problem can be solved via the multiple coprime property. Furthermore, we employ a spectral peak searching method that can exploit the whole aperture and full DOFs of the IUCLA to detect targets and achieve angle estimation. Meanwhile, the proposed method avoids extra processing in eliminating ambiguous angles, and reduces the computational complexity. Finally, the Cramer–Rao bound (CRB) and numerical simulations are provided to demonstrate the effectiveness and superiority of the proposed method.