<p>Gold tailings (GTs) contain abundant silica resources but have not received sufficient attention. Notably, their high silica content offers the possibility of serving as a sustainable alternative to natural quartz resources. This study proposes an innovative strategy for producing 4N6-grade (SiO₂ content ≥ 99.9960%) high-purity quartz (HPQ) from GTs using superconducting high-gradient magnetic separation (S-HGMS) combined with an ecofriendly two-step leaching protocol comprising low-fluorine mixed acid treatment followed by hot-pressure fluorine-free leaching. In the S-HGMS stage, a pre-enriched quartz concentrate with a SiO₂ grade of 93.97% was obtained using a magnetic flow ratio of 0.085 T·s/m, which was 15.16% higher than the SiO₂ content in GTs. This concentrate was then further purified through the two-step leaching method, resulting in HPQ with a SiO₂ content of 99.9964%. Mechanistic investigations demonstrated that quartz particles and impurity particles exhibit significantly different magnetic characteristics in the strong magnetic field generated by the S-HGMS system, thus achieving their separation. The initial low-fluorine mixed acid treatment not only dissolves and removes silicate impurities adhering to the quartz surface, but also induces the formation of corrosion pits on quartz particles, creating more favorable conditions for subsequent leaching. The hot-pressure fluorine-free leaching intensifies the erosion of quartz particles by the acid solution, increasing contact probability with internal impurities, thus enabling the deep removal of impurities. This study establishes a green technology approach to convert GTs into 4N6 HPQ products, which not only achieves high-value utilization of GTs, but also provides a novel idea for high value-added utilization of metallurgical solid waste.</p> Graphical Abstract <p></p>