Due to the high impact of the building sector on the environment, a growing interest focuses on insulating materials able to ensure good thermo-acoustic performance for the building envelope from a sustainable and circular economy perspective. In this context, Moroccan natural gypsum was mixed with local natural waste materials. The thermal and acoustic properties of the samples were measured; they were compared to those of synthetic- and mineral-based gypsum plasters manufactured with the same technique. A Small Hot Box apparatus was used for thermal characterization, whereas acoustic performance was investigated by means of a Kundt’s Tube. Natural and synthetic additives result in a reduction in density and an improvement in thermal performance. Conductivity values in the 0.181–0.238 W/mK range were obtained, depending on the type of natural additive, with respect to 0.275–0.323 W/mK of mineral-based gypsum plasters. The acoustic measurements showed that all the composites have similar performance in terms of acoustic absorption, whereas high transmission loss values were obtained for the natural additives (TL = 35–59 dB). Petiol of Palm and Stipa Tenacissima were found to be materials able to improve both thermal and acoustic properties.