The viability of incorporating agricultural by-products, such as oat husks, not yet explored in limestone-based composites, as more sustainable alternatives for use as novel aggregates may be improved through the adoption of well-known valorisation strategies applied to other plant-based resources. In this context, this work innovates by assessing how treatments on oat husk surfaces and the choice of limestone-based binders impact the mechanical performance of composites. The strategy adopted to achieve these objectives, in addition to carrying out the physical and geometric characterisation of the husks, consists of treating the husks’ surface using washing cycles in water, cement/pozzolan binder, and linseed oil. Furthermore, matrices combining cement, calcium hydroxide Ca(OH)2, and microsilica (SiO2) were used. In conclusion, even though the effects of different binder combinations are inconsistent, coating oat husks—especially with linseed oil—works well in delaying particle degradation and improving mechanical strength compared to untreated particles. Furthermore, when aggregates are substituted with the longer and lamellar particles of oat husk, the impact of the water/cement ratio on mechanical performance and composite workability significantly decreases.