Over the last two decades, there was been intensive study of pozzolans on the surface of the Los Frailes Caldera (Spain) for possible use as construction materials; however, research into the deepest underlying horizons has not yet been done. The main object of this paper is to present the results of the research carried out at different levels of depth, down to 30 m, to locate and demonstrate the presence of pozzolans in the depths of the Los Frailes Caldera. To achieve this, a series of analyses were carried out to classify the samples extracted from the various levels of depth, starting at the surface and continuing down to 30 m, which consisted of XRD, XRF, and SEM. Other technological tests were also performed such as chemical analysis of pozzolanic quality (CAQP) and pozzolanicity (PT) tests, at 8 and 15 days. Lastly, a geophysical study using electrical resistivity tomography (ERT) was developed to define the thickness and physical properties of the horizons of pozzolanic materials at depth, as well as to establish the depth of the deposit. The results obtained by XRD, XRF, and SEM confirmed the presence of pozzolans consisting of strongly zeolitized and bentonitised tuffs (ZBVT) in the lower levels of the Los Frailes Caldera, indicating that these horizons continue uninterruptedly beyond 30 m deep. The results of the CAQP and PT established that the ZBVTs that lie in the depths have pozzolanic qualities. On the other hand, the ERT study showed that ZBVT levels continue into the depths, thus proving that the lower limit of the deposit is even deeper. The results obtained in this work could have a positive impact on an increase in the reserves of pozzolanic raw materials in the researched area and could be used in the manufacture of light aggregates for mortars, concretes, and pozzolanic cements, consistent with the environment and effective in reducing CO2 emissions during the production process.