An intersymbol interference (ISI)-suppressed optical multilevel modulation technique that is applicable to a wide range of binary and multilevel signaling is proposed. It employs binary phase-shift keying modulations that are generated by Mach-Zehnder intensity modulators as basic building blocks, and complex multilevel modulations are synthesized using interferometric addition- and tandem modulations. Its feasibility and ISI suppression effect are verified in various binary and multilevel signal synthesis schemes using numerical simulations. Furthermore, the generation of ISI-suppressed zero-chirp binary and quaternary amplitude-shift keying modulations is experimentally demonstrated. Finally, its applicability to complex optical multilevel signaling is shown in the generation of a 40-Gb/s 16-level amplitude- and phase-shift keying signal, which results in 3-dB sensitivity improvement compared with the one using a conventional four-level electrical driving signal.