In this paper, a triple-layer hybrid optical orthogonal frequency division multiplexing (THO-OFDM) for intensity modulation with direct detection (IM/DD) systems with a high spectral efficiency is proposed. We combine N-point asymmetrically clipped optical orthogonal frequency division multiplexing (ACO-OFDM), N /2-point ACO-OFDM, and N /2-point pulse amplitude modulated discrete multitoned (PAM-DMT) in a single frame for simultaneous transmission. The time-and frequency-domain demodulation methods are introduced by fully exploiting the special structure of the proposed THO-OFDM. Theoretical analysis show that, the proposed THO-OFDM can reach the spectral efficiency limit of the conventional layered ACO-OFDM (LACO-OFDM). Simulation results demonstrate that, the time-domain receiver offers improved bit error rate (BER) performance compared with the frequency-domain with ∼40% reduced computation complexity when using 512 subcarriers. Furthermore, we show a 3 dB improvement in the peak-to-average power ratio (PAPR) compared with LACO-OFDM for the same three layers.