Land use and land cover (LULC) change in tropical regions can cause huge amounts of carbon loss and storage, thus significantly affecting the global climate. Due to the differences in natural and social conditions between regions, it is necessary to explore the correlation mechanism between LULC and carbon storage changes in tropical regions from a broader geographical perspective. This paper takes Hainan Island as the research object, through the integration of the CA-Markov and Integrated Valuation of Ecosystem Services and Tradeoffs (InVEST) models, based on multi-source data, analyses the dynamics of LULC and carbon storage from 1992 to 2019 and the relationship between the two, and predicts future LULC and carbon storage under different scenarios. The results show that (1) the built-up land area of Hainan Island expanded from 103.59 km2 to 574.83 km2 from 1992 to 2019, an increase of 454.91%; the area of cropland and shrubland decreased; and the area of forest increased. (2) Carbon storage showed an upward trend during 1992–2000, and a downward trend during 2000–2019. Overall, LULC changes during 1992–2019 reduced carbon storage by about 1.50 Tg. (3) The encroachment of cropland in built-up land areas is the main reason for the reduction of carbon storage. The conversion of shrubland to forest is the main driving force for increasing carbon storage. The increase and decrease of carbon storage have obvious spatial clustering characteristics. (4) In the simulation prediction, the natural trend scenario (NT), built-up land priority scenario (BP) and ecological priority scenario (EP) reduce the carbon storage of Hainan Island, and the rate of decrease is BP> NT > EP. The cropland priority scenario (CP) can increase the LULC carbon storage, and the maximum increase in 2050 can reach 0.79 Tg. This paper supplements and improves the understanding of the correlation between LULC and carbon storage changes in tropical regions, and can provide guidance for the optimization of LULC structure in tropical regions with high economic development from a low-carbon perspective.