The orthogonal frequency-division multiplexing (OFDM) mode with a linear frequency modulation (LFM) signal as the baseband waveform has been widely studied and applied in multiple-input multiple-output (MIMO) radar systems. However, its high sidelobe levels after pulse compression affect the target detection of radar systems. For this paper, theoretical analysis was performed, to investigate the causes of high sidelobe levels in OFDM-LFM waveforms, and a novel waveform optimization design method based on deep neural networks is proposed. This method utilizes the classic ResNeXt network to construct dual-channel neural networks, and a new loss function is employed to design the phase and bandwidth of the OFDM-LFM waveforms. Meanwhile, the optimization factor is exploited, to address the optimization problem of the peak sidelobe levels (PSLs) and integral sidelobe levels (ISLs). Our numerical results verified the correctness of the theoretical analysis and the effectiveness of the proposed method. The designed OFDM-LFM waveforms exhibited outstanding performance in pulse compression and improved the detection performance of the radar.