Fluorine (F) enrichment originating from natural sources is difficult to remove using chemical washing methods due to the large chemical-resistant residual fraction. This study evaluates the feasibility of using a froth-flotation separation method to remediate soil with a high F concentration caused by mica weathering, and it investigates the optimal conditions for this process, including pH of the slurry, collector dosage, and sample mechanical preparation strategy. The established optimum conditions are pH 3.5, 300 mg/kg collector dosage (tallow amine acetate), which can effectively separate quartz and mica, and a sieving-and-milling strategy that involves discarding particles of size < 0.05 mm, milling those in the range of 0.5–2.0 mm (until < approx. 0.3 mm), and mixing particles with sizes in the range of 0.05–0.5 mm. The target contamination level of 400 mg/kg for the test soil was not met after the first flotation separation process. However, after milling the residue of the first process and subjecting it to a second flotation separation process, the required contamination level was achieved. Consequently, the proposed froth-flotation separation process can be used as a successful alternative technique to remediate F-enriched soils from natural origin that have highly chemical-resistant forms.