This paper reports a study on 8 unconventional hydraulic lime-based mortars able to improve indoor air quality by acting as passive systems. Mortars have been prepared with commercial sand or highly adsorbent materials as aggregates with/without TiO2 as photocatalytic agent, to test also the decomposition of airborne pollutants. Mechanical properties, hygrometric behavior, inhibition of growth of molds and depollution properties have been tested. Despite using porous materials (zeolite and activated carbon), in mortars with unconventional aggregates, compressive strength is higher than in sand-based ones, with a more than double higher water vapor permeability. Zeolite-based mortars have the highest moisture buffering capacity followed by silica gel- and activated carbon-based mortars (1.5–2 times higher than reference, respectively, because of the high porosity of unconventional aggregates). Sand-based mortars show optimum inhibitory capacity against fungal growth. Concerning unconventional aggregates, silica gel mortars have good inhibitory capacity, whereas zeolite and activated carbon give to mortars an optimum substrate for molds. Mortars with unconventional aggregates as silica gel remove more than 80% of tracer pollutant after 2 h of test, whereas zeolite-based mortars remove the 65% of it after 120 min. TiO2 enhances depollution properties as photocatalytic oxidation agent when the mortar is close to saturation.