In this paper, an approach to generate frequency-doubling sinc-shaped optical Nyquist pulses based on external modulation is proposed and demonstrated. First, four flat optical frequency comb (OFC) lines are obtained after optical carrier suppression modulation in a dual-electrode Mach-Zehnder modulator. Then an optical interleaver is introduced to split the phase-locked OFC into two paths, of which one is transmitted to a dual-parallel Mach-Zehnder modulator for quadrupling RF modulation and another is applied to the remodulated signal to acquire comb lines with equal intervals. Thus, a phase-locked 12-line flat OFC with equal frequency intervals and corresponding Nyquist pulses is finally obtained, and Nyquist pulses at 2.5GHz, 5GHz, 10GHz, and 15GHz are achieved.