Cross-laminated timber (CLT) is one of the most sustainable, robust, and green building materials nowadays and is normally used for walls, floors, or roofs. The number of studies on CLT has increased significantly since 2010, which shows the acceptance and needs of CLT. Connection systems, rolling shear performance, and sustainability are the popular and main research topics within CLT, including wooden connections, metallic connections, adhesive and rod connections, aspect ratio, bonding performance, life cycle assessment, carbon emission, and environmental impact. Based on these three branches, the current study conducts a literature review on CLT. This review article aims to provide a valuable view and better understanding of CLT, which are linked to (1) promoting the usage of CLT and (2) summarizing the weaknesses of the CLT’s research. This article presents a full background of the CLT research and gives potential research directions for CLT as a structural material. It revealed that the design and analytical methodologies for novel timber and steel connections are the main trends. As for the CLT’s rolling shear performance, standardized testing protocol, environmental impact, and bonding quality need further development. Furthermore, the data collection, selection, and influence of different policies are important for the CLT’s sustainability assessment.