We present new generation and detection methods for high symbol-rate 64-ary quadrature amplitude modulation (64QAM). The 64QAM signal is created by tandem in-phase/quadrature (I/Q) modulators driven by electrical binary signals. The first I/Q modulator, which has four drive arms (i.e. a dual-drive I/Q modulator), yields 16QAM with an offset at the 1st quadrant of the complex plane. Subsequently, the second modulator switches this 16QAM signal over four quadrants via the typical quadrature phase-shift-keying (QPSK) modulation scheme, hence the desired 64QAM is generated. To mitigate the impacts of transmitter imperfections, we also propose a phase-folded decision-directed (PF-DD) linear equalizer at the receiver. Using these new techniques, we experimentally demonstrate the 120- and 240-Gb/s polarization-division-multiplexed (PDM) return-to-zero (RZ) 64QAM systems. The required optical signal-to-noise ratio (OSNR) for a bit-error rate (BER) of 2.4x10(-2) is measured at 20.2 or 23 dB, respectively, which is ~3.5 dB off the theoretical limit.