Altered pyroclastic (tephra) deposits are highly susceptible to landsliding, leading to fatalities and property damage every year. Halloysite, a low-activity clay mineral, is commonly associated with landslide-prone layers within altered tephra successions, especially in deposits with high sensitivity, which describes the post-failure strength loss. However, the precise role of halloysite in the development of sensitivity, and thus in sudden and unpredictable landsliding, is unknown. Here we show that an abundance of mushroom cap–shaped (MCS) spheroidal halloysite governs the development of sensitivity, and hence proneness to landsliding, in altered rhyolitic tephras, North Island, New Zealand. We found that a highly sensitive layer, which was involved in a flow slide, has a remarkably high content of aggregated MCS spheroids with substantial openings on one side. We suggest that short-range electrostatic and van der Waals interactions enabled the MCS spheroids to form interconnected aggregates by attraction between the edges of numerous paired silanol and aluminol sheets that are exposed in the openings and the convex silanol faces on the exterior surfaces of adjacent MCS spheroids. If these weak attractions are overcome during slope failure, multiple, weakly attracted MCS spheroids can be separated from one another, and the prevailing repulsion between exterior MCS surfaces results in a low remolded shear strength, a high sensitivity, and a high propensity for flow sliding. The evidence indicates that the attraction-detachment model explains the high sensitivity and contributes to an improved understanding of the mechanisms of flow sliding in sensitive, altered tephras rich in spheroidal halloysite.