Focusing on how to improve the system spectral efficiency of Prolate Spheroidal Wave Functions( PSWFs) multi-carrier modulation system, a third constellation composed of additional constellation points on the basis of multi-carrier index modulation based on PSWFs with dual-mode method is introduced in this paper. The Multi-Carrier index Modulation based on PSWFs with Better multIple-Mode (BIM- MCM-PSWFs) is proposed. In this method, the signal index dimension is expanded and the number of modulation symbol combinations is increased through the multiple arrangement and combination of subcarriers in each sub block after grouping. The method proposed in this paper realizes the further utilization of spectrum resources in the multi-carrier index modulation based on PSWFs with dual-mode method, and improves effectively system spectral efficiency. Theoretical and simulation analysis show that, compared with the multi-carrier index modulation based on PSWFs with dual-mode method, the method proposed in this paper has a higher system spectral efficiency at the cost of appropriately sacrificing bit error performance. When n=9, k=1, m=4, Spectral Efficiency(SE) is increased by 20.1% at the expense of 0.70 dB of Bit Error Rate(BER).