High accuracy and reliable predictions of the bias of in-orbit atomic clocks are crucial to the application of satellites, while their clocks cannot transfer time information with the earth stations. It brings forward a new short-term, mid-long-term, and long-term prediction approach with the grey predicting model (GM(1, 1)) improved by the least absolute deviations (GM(1, 1)-LAD) when there are abnormal cases (larger fluctuations, jumps, and/or singular points) in SCBs. Firstly, it introduces the basic GM(1, 1) models. As the parameters of the conventional GM(1, 1) model determined by the least squares method (LSM) is not the best in these cases, leading to magnify the fitting errors at the abnormal points, the least absolute deviations (LAD) is used to optimize the conventional GM(1, 1) model. Since the objective function is a nondifferentiable characteristic, some function transformation is inducted. Then, the linear programming and the simplex method are used to solve it. Moreover, to validate the prediction performances of the improved model, six prediction experiments are performed. Compared with those of the conventional GM(1, 1) model and autoregressive moving average (ARMA) model, results indicate that (1) the improved model is more adaptable to SCBs predictions of the abnormal cases; (2) the root mean square (RMS) improvement for the improved model are 5.7%∼81.7% and 6.6%∼88.3%, respectively; (3) the maximum improvement of the pseudorange errors (PE) and mean absolute errors (MAE) for the improved model could reach up to 88.30%, 89.70%, and 87.20%, 85.30%, respectively. These results suggest that our improved method can enhance the prediction accuracy and PE for these abnormal cases in SCBs significantly and effectively and deliver a valuable insight for satellite navigation.