Tensor train (TT) factorization and corresponding TT rank, which can well express the low-rankness and mode correlations of higher-order tensors, have attracted much attention in recent years. However, TT factorization based methods are generally not sufficient to characterize low-rankness along each mode of third-order tensor. Inspired by this, we generalize the tensor train factorization to the mode-k tensor train factorization and introduce a corresponding multi-mode tensor train (MTT) rank. Then, we proposed a novel low-MTT-rank tensor completion model via multi-mode TT factorization and spatial-spectral smoothness regularization. To tackle the proposed model, we develop an efficient proximal alternating minimization (PAM) algorithm. Extensive numerical experiment results on visual data demonstrate that the proposed MTTD3R method outperforms compared methods in terms of visual and quantitative measures.