Parameter estimation of the lunar regolith not only provides important information about the composition but is also critical to quantifying potential resources for lunar exploration and engineering for human outposts. The Lunar Penetrating Radar (LPR) onboard China’s Chang’E-3 (CE-3) provides a unique opportunity for mapping the near-surface stratigraphic structure and estimating the parameters of the regolith. In this paper, the electrical parameters and the iron-titanium content of regolith are estimated based on the two sets of LPR data. Firstly, it is theoretically verified that the relative dielectric constant can be estimated according to the difference of the reflected time of two receivers from a same target. Secondly, in order to verify the method, a parameter estimation flow is designed. Subsequently, a simple model and a complex model of regolith are carried out for the method verification. Finally, on the basis of the two sets of LPR data, the electrical parameters and the iron-titanium content of regolith are estimated. The relative dielectric constant of regolith at CE-3 landing site is 3.0537 and the content of TiO2 and FeO is 14.0127%. This helps us predict the reserves of resources at the CE-3 landing site and even in the entire Mare Imbrium.