Light scattering method is the most commonly used method for on-line measurement of ultralow particulate matter mass concentration. However, when the particle characteristics change, the effectiveness of the empirical relationship decreases, which would lead to a sizeable deviation. To accurately measure the mass concentration of particulate matter in real-time, a coupling measurement idea of light scattering and beta-ray attenuation is proposed. The beta-ray attenuation is little affected by particle properties and accurately reflects the average PM mass concentration in the measured period. The single calibration method (M1), periodic calibration method (M2), average calibration method (M3), and asymmetric factor calibration method (M4) are formed based on the coupling idea. The results of all methods are perfect when the particle size is unchanged. However, when the particle sizes fluctuate frequently, the results of M1, M2, and M3 deviate seriously from the actual value, and the applicable working conditions have limitations. The results of M4 are in good agreement with the actual value, and the effectiveness is not limited by the particle size. Finally, the prototype based on experimental exploration was developed and had been continuously operated for more than 528 h at a 1000 MW unit of a coal-fired power plant.