This work mainly focuses on the off-axis compressive behavior of cross-laminated bamboo and timber (CLBT) wall elements. In total, 224 off-axis specimens were tested, which were made from hem-fir lumber and bamboo mat-curtain panels or just hem-fir lumber. Based on the in-plane compressive failure criteria and prediction models for the off-axis apparent compressive modulus, the mechanical property parameters of the off-axis tests were predicted. Experimental results showed that the main failure modes were slender failure zones along the parallel or perpendicular to the off-axis angles and delamination failures between the layers. The orthogonal structures inside the off-axis specimens dispersed the compressive performance of the major strength direction. Compared with glued-laminated timber specimens, the off-axis compressive performance of cross-laminated timber and CLBT specimens varied more smoothly with the increase of the off-axis angle. In addition, the characteristics of the model forms and materials affected the accuracy of the off-axis compressive property prediction models. The results in this paper can provide some inspiration for a series of innovative full-size CLBT wall members.