Zeolites are a class of materials that are of great relevance for industrial catalysis. Several fundamental questions relating to the structure and role of the Lewis acid sites in these materials remain unanswered. Proposals for the origin of such species can broadly be classified into three categories, which have distinct structures: extra-framework, framework-associated and framework aluminium. In this Perspective, we review each of these proposals and proceed to analyse their suitability to understand experimental results. Contrary to traditional belief, the number of Lewis acid sites does not always correlate to extra-framework aluminium content. As a result, we highlight that the terms 'extra-framework' and 'framework-associated' aluminium should be used with caution. We propose how the usage of different characterization techniques can enable the closure of knowledge gaps concerning the strength, multiplicity, localization and structure of catalytically active Lewis acid sites in zeolites. Lewis acid aluminium sites in zeolites enable some industrially relevant catalytic reactions, such as biomass valorization. This Perspective explores the origin and interpretation of these species, and discusses characterization techniques that can close knowledge gaps.