Cr1-xTixO2 (0 ≤ x ≤ 1) solid solution was synthesized by a high-pressure and high-temperature method, whereafter systematic experimental and computational studies were conducted on the Cr1-xTixO2 system. The crystal structure of the samples where 0 ≤ x ≤ 0.4 and x = 1 was of a rutile structure (P42/mnm), while samples where 0.5 ≤ x ≤ 0.9 crystallized in a CaCl2 structure (Pnnm). The structural transformation from rutile-type to CaCl2-type structure should be due to the combined action of positive chemical pressure and physical pressure. The saturation magnetization of the Cr1-xTixO2 samples decreased linearly with the increase of x because Ti4+ is nonmagnetic. In addition, the Curie temperature of the Cr1-xTixO2 samples also decreased noticeably with the increase of x. When nonmagnetic Ti4+ randomly replaced Cr4+ and occupied its position, the net exchange coupling in Cr1-xTixO2 would decrease. When Ti4+ occupied the majority in the system, Cr4+ ions would be separated by nonmagnetic Ti4+ ions far enough for the long-range ferromagnetic order to weaken or even disappear with the increase of x, causing the Cr1-xTixO2 system to finally approach a paramagnetic state. Density functional theory calculations were performed for the Cr1-xTixO2 system, and the predicted trends of the magnetic properties agreed well with the experimental results. These calculations also showed that Cr1-xTixO2 was still half-metallic until x reached 0.6.