The European Commission adopted a long-term strategic vision aiming for climate neutrality by 2050. Lithuania ratified the Paris agreement, making a binding commitment to cut its 1990 baseline GHG emissions by 40% in all sectors of its economy by 2030. In Lithuania, the main construction material is cement, even though Lithuania has a strong wood-based industry and abundant timber resources. Despite this, approximately twenty percent of the annual roundwood production from Lithuanian forests is exported, as well as other final wood products that could be used in the local construction sector. To highlight the potential that timber frame construction holds for carbon sequestration efforts, timber and concrete buildings were directly compared and quantified in terms of sustainability across their production value chains. Here the concept of “exemplary buildings” was avoided, instead a “traditional building” design was opted for, and two- and five-floor public buildings were selected. In this study, eleven indicators were selected to compare the sustainability impacts of wood-based and concrete-based construction materials, using a decision support tool ToSIA (a tool for sustainability impact assessment). Findings revealed the potential of glue-laminated timber (GLT) frames as a more sustainable alternative to precast reinforced concrete (PRC) in the construction of public low-rise buildings in Lithuania, and they showed great promise in reducing emissions and increasing the sequestration of CO2. An analysis of environmental and social indicators shows that the replacement of PRC frames with GLT frames in the construction of low-rise public buildings would lead to reduced environmental impacts, alongside a range of positive social impacts.