Low-carbon buildings and construction products can play a key role in creating a low-carbon society. Cross-laminated timber (CLT) is proposed as a prime example of innovative building products, revolutionising the use of timber in multi-storey construction. Therefore, an understanding of the synergy between structural engineering design solutions and climate impact of CLT is essential. In this study, the carbon footprint of a CLT multi-storey building is analysed in a life cycle perspective and strategies to optimise this are explored through a synergy approach, which integrates knowledge from optimised CLT utilisation, connections in CLT assemblies, risk management in building service-life and life cycle analysis. The study is based on emerging results in a multi-disciplinary research project to improve the competitiveness of CLT-based building systems through optimised structural engineering design and reduced climate impact. The impacts associated with material production, construction, service-life and end-of-life stages are analysed using a process-based life cycle analysis approach. The consequences of CLT panels and connection configurations are explored in the production and construction stages, the implications of plausible replacement scenarios are analysed during the service-life stage, and in the end-of-life stage the impacts of connection configuration for post-use material recovery and carbon footprint are analysed. The analyses show that a reduction of up to 43% in the life cycle carbon footprint can be achieved when employing the synergy approach. This study demonstrates the significance of the synergy between structural engineering design solutions and carbon footprint in CLT buildings.