This study proposes an eco-friendly approach to zeolite agglomeration for petroleum sorbents. The novelty lies in integrating agglomeration and deagglomeration within a single high-pressure grinding roll (HPGR) system, enhancing sorption capacity by creating a secondary porosity network. This eliminates energy-intensive calcination, making it a sustainable alternative to wet granulation. We examine the impact of binder and water dosages on sorption capacity, mechanical resistance, and textural properties of roll-compacted zeolite agglomerates. Feed materials were characterized using N₂ adsorption, XRD, XRF, particle size distribution, and SEM. Structural and functional properties were assessed via mercury intrusion porosimetry, petroleum sorption efficiency (Westinghouse test), sorption capacity, gravitational drop tests, and SEM. All sorbents (0.5–1 mm) met the 50 wt.% oil absorbency threshold for petroleum spill cleanup in Poland. The fabricated zeolite agglomerates exhibited superior sorption capacities compared to zeolite powder, Na-P1, and commercial sorbents. The optimal feed composition yielded sorbents with the best properties and versatile performance. An analysis of sorption characteristics and pore size distribution showed that a higher proportion of 10–100 µm pores improved efficiency. This study addresses the knowledge gap in zeolite powder agglomeration and demonstrates the effectiveness of integrating agglomeration and deagglomeration in a high-pressure roller press.