In iron and steel sintering production, traditional granulation processes often face poor particle aggregation uniformity and high residual fine content, which leads to large fluctuations in the permeability of the sinter bed and uneven thermal reactions. To address these issues, this study innovatively integrates the granulation process using external rolling of coke powder and quicklime with pre-wetting treatment. The study systematically explores the coupling effects of granulation moisture, rotation speed, lime addition, coke powder particle size, and pre-wetting time with carbon content and moisture in the sintering mixture. Experimental results indicate that granulation with 7%–8% moisture, 22–24 r/min rotation speed, 3.5% lime addition, 1.5–2.0 mm average coke powder size, and 3 min pre-wetting time, combined with 3.8% carbon content in the sintering step, produces granules with excellent sphericity. Under these conditions, drum strength of the sintered ore reaches 66.2%, and reduction performance is significantly improved, meeting the requirements for high-quality sintered ore. In summary, the proposed improved process and full-process parameter experimental method provide an effective approach to address the chain problem of “poor granule quality–low sintering efficiency–fluctuating ore performance” in traditional sintering. This study not only supports steel enterprises in improving sintering efficiency and reducing energy consumption but also ensures the stable supply of high-strength, high-reducibility sinter to blast furnaces, promoting more efficient and greener steel production.