The growing concerns for the environmental impact of resource depletion and carbon emissions has led to the current study of using novel, sustainable materials in natural rubber compounds. The principal goal of this study was to reduce the usage of the non-renewable filler carbon black (CB). For this purpose, two waste-derived calcium carbonates were introduced in natural rubber compounds as a partial replacement for CB. To enhance their performance, the compounds were modified using alpha-lipoic acid and a titanate as in situ coupling agents. The effect of these renewable fillers and coupling agents on the in-rubber properties was analyzed using various characterization methods. Remarkably, by replacing 10 phr of carbon black with a calcium carbonate filler and introducing the alpha-lipoic acid coupling agent, a compound was obtained with performance levels similar to the CB-filled reference compound. These findings contribute valuable insights into the replacement of carbon black with renewable calcium carbonate fillers.