This article proposes and experimentally demonstrates a radio-over-fiber system employing single-sideband single-carrier (SSB-SC) modulation at 60 GHz. SSB-SC modulation has a lower peak-to-average-power ratio than orthogonal frequency division multiplex (OFDM) modulation; therefore, the SSB-SC signals provide superior nonlinear tolerance, compared to OFDM signals. Moreover, multiple-input multiple-output (MIMO) technology was used extensively to enhance spectral efficiency. A least-mean-square-based equalizer was implemented, including MIMO channel estimation, frequency response equalization, and I/Q imbalance compensation to recover the MIMO signals. Thus, using 2 × 2 MIMO technology and 64-QAM SSB-SC signals, we achieved the highest data rate of 84 Gbps with 12 bit/s/Hz spectral efficiency using the 7-GHz license-free band at 60 GHz.