Halloysite nanotubes, a naturally occurring nanomaterial with a unique tubular morphology, have shown considerable potential for heavy metal remediation. However, significant inconsistencies in the reported maximum adsorption capacities (q_max) for heavy metal ions—such as Pb²⁺, which ranges from 7.5 to 84.0 mg/g with a coefficient of variation (CV) of 68%—have severely hindered both scientific understanding and practical application of this promising material. To address this critical knowledge gap, we conducted a reassessment using carefully selected halloysite specimens from three geologically distinct deposits (Utah, USA; Henan and Yunnan, China). Under rigorously controlled experimental conditions, we precisely quantified the adsorption capacities of halloysite for Cd²⁺, Zn²⁺, and Pb²⁺. Through an integrated multi-technique characterization approach involving XRF, XRD, FTIR, TEM, and BET analyses, we identified two fundamental crystallochemical parameters that govern the adsorption performance of halloysite: the degree of lattice substitution and the density of surface hydroxyl groups. Our findings reveal that optimal heavy metal adsorption occurs in halloysite with lower lattice substitution and higher surface hydroxyl density. This work not only provides a reliable range of adsorption capacities for halloysite but, more importantly, establishes a scientific foundation for optimizing the application of halloysite in heavy metal remediation.