Spectral computed tomography (CT) can divide collected photons into multi-energy channels and gain multi-channel projections synchronously by using photon-counting detectors. However, reconstructed images usually contain severe noise due to the limited number of photons in the corresponding energy channel. Tensor dictionary learning (TDL)-based methods have achieved better performance, but usually lose image edge information and details, especially from an under-sampling dataset. To address this problem, this paper proposes a method termed TDL with an enhanced sparsity constraint for spectral CT reconstruction. The proposed algorithm inherits the superiority of TDL by exploring the correlation of spectral CT images. Moreover, the method designs a regularization using the L0-norm of the image gradient to constrain images and the difference between images and a prior image in each energy channel simultaneously, further improving the ability to preserve edge information and subtle image details. The split-Bregman algorithm has been applied to address the proposed objective minimization model. Several numerical simulations and realistic preclinical mice are studied to assess the effectiveness of the proposed algorithm. The results demonstrate that the proposed method improves the quality of spectral CT images in terms of noise elimination, edge preservation, and image detail recovery compared to the several existing better methods.