In a Fourier transform infrared (IR) spectrometer, the Michelson interference signal extrapolation method based on linear prediction is often used to improve spectral resolution. In this method, an autoregressive (AR) model is established for the Michelson interference signal in the spectrometer. Once the AR model parameters are determined, the AR process is predictable. The interference signal can be used to figure out the AR model's parameters. Based on this, the AR model can be used to extrapolate the interference signal to improve the spectral resolution. In this paper, the forward–backward linear prediction total least squares (FB-TLS) method is proposed to estimate the parameters of the AR model. The parameters that are estimated are used to improve the IR spectral resolution. By simulating different order and signal-to-noise ratio situations, the effects of the Burg, the least square, and the FB-TLS parameter estimation methods on spectral resolution enhancement are studied. The simulation results demonstrate that the FB-TLS parameter estimation method can effectively suppress noise and avoid spurious peaks. The experimental results demonstrate that the FB-TLS parameter estimation method is effective for spectral resolution enhancement technology based on linear prediction. When the FB-TLS method is used to enhance NH3 IR spectral resolution from 2 cm−1 to 1 cm−1, the spectral prediction error in the NH3 characteristic band is only 0.21% compared with the measured NH3 spectrum, whose spectral resolution is 1 cm−1.