The land-use, land-use change and forestry (LULUCF) sector is receiving increasing attention in climate change mitigation and greenhouse gas (GHG) emission offsetting. The sector itself and measures applied to mobilize this sector in order to tackle climate change are dominant in nationally determined contributions under the Paris Agreement as well as in national strategies, as in the case of Lithuania. Lithuania has set the goal of becoming a carbon-neutral country in 2050, reducing GHGs by 80% compared to 1990 and offsetting the remaining 20% through the LULUCF sector. Therefore, this paper aims at analyzing historical land-use changes in 1990–2021, as reported for the United Nations Framework Convention on Climate Change (UNFCCC) secretariat, and LULUCF’s potential to achieve climate change mitigation goals, taking into account different land-use change scenarios (business as usual, forest development, forest development + additional measures and forest land 40% + additional measures) for 2030 and 2050 in Lithuania. The scenarios are based on historical and potential future policy-based land-use changes. Projections of GHG emissions/removals for different scenarios are prepared according to the Good Practice Guidance and Uncertainty Management in National Greenhouse Gas Inventories (2006) by the Intergovernmental Panel on Climate Change (IPCC). The results indicate that land-use changes over the period 1990–2021 remained rather stable, with some increases in forest area and grassland at the expense of cropland. The whole LULUCF sector acted as a carbon sink in most cases, forests being a key category for removal. However, reaching climate neutrality in 2050 might be challenging, as the goal to offset 20% of remaining GHG emission compared to 1990 through LULUCF would not be met in any of the scenarios analyzed, even the scenario of maximal forest-area development and additional measures. Considering the high historical GHG-removal fluctuations and the uncertainties of the sector itself, caution should be taken when relying on LULUCF’s potential to reach the set goals.