As a result of low porosity and low permeability in tight reservoirs, spontaneous imbibition plays an important role in oil recovery. While wettability has a crucial impact on the imbibition, the mechanism of the effect of wettability on imbibition is still unclear. In this study, we screened the surfactants with similar interfacial tension (IFT) at the same concentration to study the wettability properties, which will contribute to improve the oil recovery tight reservoir. Two betaine surfactants, lauramide propyl hydroxysulfonated betaine (LHSB) and cocamidopropyl betaine (CAB), were screened according to their IFT. Through spontaneous imbibition experiments, the recovery of LHSB (27.26%) was better than that of CAB (21.69%). The contact angle method and U.S. Bureau of Mines method were used to analyze the core wettability comprehensively. After LHSB treatment, the core wettability index turned to hydrophobic and the wettability index changed from -0.06 to -0.56. However, the wettability index did not change significantly after CAB treatment (-0.15). Further molecular simulations showed that, after the surface of the rock is modified by LHSB, the oil droplets spread gradually and the interface energy with the quartz was enhanced. In combination of the analysis of the. potential and adsorption measurement, LHSB is predicted to be adsorbed in a single-layer configuration, while CAB formed a double-layer configuration, which caused the difference in wettability. It can be speculated that, when the surfactant changes the pore surface of the tight sample toward hydrophobic, the oil-wet surface promotes the residual oil droplets to form a continuous phase and, at the same time, reduces flow resistance of the water phase, thereby increasing the spontaneous imbibition rate and the ultimate recovery. This study will help to understand the wettability impact on imbibition by the surfactant and contribute to the improvement of tight oil reservoir recovery.