The invention discloses a method for making high-square-degree sintered NdFeB permanent magnets with a cerium, titanium, cobalt and zirconium compound additive. The method comprises the steps that raw materials are prepared with 27.0% to 29.0% of Nd, 2.5% to 4.0% of Ce, 63.5% to 67.5% of Fe, 1.0% to 1.2% of B, 0.5% to 1.0% of Nb, 1.0% to 3.0% of Co, 0.1% to 0.3% of Zr, 10.5% to 1.0% of A, 0.1% to 0.3% of Cu, and 0.1% to 0.3% of Ti, the raw materials are smelted under the temperature of 1380 DEG with a vacuum induction rapid-hardening casting strip furnace, smelted alloy liquid is processed through electromagnetic stirring to be uniform, and is poured to a rotating water-cooling copper stick, and the alloy liquid is rapidly cooled to form alloy slices with the thickness ranging from 0.2 mm to 0.5 mm; NdFeB alloy slices are broken into NdFeB alloy particles with the length ranging from 120 microns to 200 microns with a hydrogen breaking furnace; the particles are further broken into NdFeB alloy powder with the length ranging from 3.0 microns to 4.5 microns by an air-current mill; the powder is formed in a forming press, and is further densified through isostatic cool pressing; formed initial blanks are sintered, and sintered permanent magnets are finally obtained. With the method for making high-square-degree sintered NdFeB permanent magnets with the cerium, titanium, cobalt and zirconium compound additive, the squre degree of the permanent magnets can be improved, and the production cost can be greatly reduced.