Nyquist signals with low roll-off factors pose a challenge for non-data-aided blind symbol rate estimation problems in long-haul applications. We adopted the nonlinear least squares (NLS) approach to estimate the symbol rate of low roll-off factor signals. This method tolerates chromatic dispersion and additive Gaussian noise. In addition, this method can operate below two samples per symbol, thus enabling low-power-consumption receivers. Simulation and experimental results show that the mean squared error is below $10^{-4}$ with only 3000 samples needed for polarization-division-multiplexed (PDM) quadrature phase-shift keying (QPSK) or quadrature amplitude modulation (QAM) systems with a roll-off factor below 0.1 for an optical signal-to-noise ratio greater than 12 dB. Compared with the maximum likelihood estimation (MLE) method, our proposed method has a more robust performance under low roll-off factor signals and in low-sampling-rate scenarios. The mean squared error remains the same for a nominal symbol rate (i.e., the ratio of the symbol rate to the sampling rate, also widely known as oversampling rate) ranging from 0.1 to 0.9.