The direct preparation of LiNi0.8Co0.1Mn0.1O2 (LNCM811) cathode materials from the hydrochloric acid leaching of laterite are promising; however, there are Cl− ions and other impurities in the hydrochloric acid leaching solution, thereby limiting the commercial application of LNCM811. In this study, we compared the LNCM811 prepared from Cl−- and SO42−- ion precursor solutions, and observed that the existence of Cl− ions could result in agglomerate disjointed and the primary particles grew separately during the sintering process, further deteriorating the electrochemical performance. Therefore, the initial raw Ni/Co solid residues were washed with deionised water and leached with 25 wt% H2SO4 solution to obtain an enriched Ni/Co solution with SO42− anions. Furthermore, considerable impurities in the enriched Ni/Co solution caused primary particle separation during the sintering process and led to the LNCM811 having poor electrochemical properties. Therefore, it was further purified by extraction with Cyanex272 to obtain a pure NiSO4 solution. The impurities in the NCM811 precursor prepared from this pure NiSO4 solution were below standard limits, the corresponding lithiated cathode delivers an initial reversible capacity of 192.1 mAh g−1 at 0.1C with an initial Coulombic efficiency of 86.5%; it retains 85.1% of its capacity after 100 cycles at 1.0C in 2.8–4.3 V, thereby achieving the standard of commercial LNCM811. On this basis, combined with the previous research of our group, high-value utilisation of laterite for preparing cathode materials includes the following processes: hydrochloric acid leaching, preliminary purification, alkaline oxidation precipitation, conversion of the Cl− solution system to the SO42− ion solution system, extraction, solution-phase synthesis, and calcination. Moreover, compared with the conventional process of preparing NCM811 from metal sulfates, the cost saving through the proposed process was found to be approximately 265.8 $/ton.