The forming of adsorbent powder is the bottleneck of the current technology for lithium adsorption from brine. In this study, an epoxy resin (E-12) was directly adopted to prepare a cylindrical granular adsorbent (the EP/HMO composite) with excellent adsorption performance. Furthermore, the conventional adsorption–desorption process was optimized to improve the adsorptive efficiency for lithium. The batch experimental results showed that the adsorptive capacity for lithium per gram of granular adsorbents was 30.2 mg g–1, disclosing the highest uptake of lithium reported in the literature to our knowledge. The continuous adsorption–desorption experimental results presented that the adsorptive capacities for lithium in LiCl solution and sampled brine were 21.3 mg g–1HMO and 17.2 mg g–1HMO, respectively. Moreover, 30 cyclic adsorption–desorption experiments were carried out under optimized operating conditions. The lithium recovery rate of the optimized method was 2.34 times higher than that of the conventional method, which was beneficial for the industrial application of adsorption with a packed column.