A challenge in hard rock lithium processing is the loss of fine spodumene particles to tailings during desliming. At typical west Australian lithium sites, particles finer than 45 μm are classified as non recoverable. Conventional froth flotation is inefficient for particles below approximately 38 μm due to poor particle–bubble collision efficiency. Flocculation-flotation is a promising approach of aggregating fine particles to sizes more amenable to recovery by flotation. This study demonstrates selective flocculation-flotation as a viable approach to recover fine spodumene (d50 ∼ 22 μm) from synthetic spodumene–quartz mixtures. Calcium ions serve as a dual activator, promoting sodium oleate (NaOl) and anionic polyacrylamide (PAM) flocculant adsorption onto spodumene surfaces to produce selective aggregates of approximately 100 μm, within the optimal size range for bubble–particle attachment. A key innovation is premixing PAM with NaOl before addition to the flotation pulp. Contact angle measurements show that premixed delivery raises the spodumene contact angle to 60.8° versus approximately 45° under sequential addition, while quartz surfaces remain near 45° and are not effectively recovered. Premixing shifts reagent adsorption from competitive to cooperative, with the preformed polymer–NaOl complexes promoting co-adsorption that neither reagent achieves alone in sequential dosing. Optimal conditions were identified at pH 8.5, 625 g/t Ca(II), 6000 g/t NaOl, and 80 g/t PAM at high anionic charge. Spodumene recovery increased from 25 per cent (grade 82 per cent; 6.6 per cent Li2O) without polymer to 72 per cent (grade 70 per cent; 5.6 per cent Li2O); a nearly threefold improvement while maintaining commercially relevant grade. Higher polymer charge densities selectively excluded quartz from aggregates via electrostatic repulsion, improving concentrate grade without sacrificing recovery. All results used commercially available polymers (Syensqo Cyfloc and BASF Alclar series) and standard flotation equipment, establishing a clear pathway to industrial scale-up. The approach offers a meaningful opportunity to improve lithium yield, reduce tailings volumes, and strengthen the sustainability of Australian spodumene operations.