At a strategic moment for agricultural soils, which are expected to contribute to climate change mitigation through carbon storage while safely feeding a growing world population, the fertiliser strategies used will be key. In a calcareous soil with extensive rainfed agricultural use and straw removal, different fertiliser strategies were evaluated with the aim of determining their effects on crop yield, nitrogen agronomic efficiency, and the storage of organic carbon and total nitrogen in the soil. Different doses of mineral fertiliser, expressed as kg of mineral nitrogen ha−1 year−1 (0, 60, 120, 180, and 240 nitrogen fertilising units (NFUs)), were applied to plots with and without biosolid amendment. The biosolid, applied at a rate of 40 Mg ha−1 every 3 years for 18 years, complied with national and European regulations to be applied on agricultural soil. The use of combined fertilisation reduced the amount of mineral fertiliser applied between 33 and 67% and the total fertiliser units between 7 and 40%, while maintaining similar yields to the reference mineral fertilisation (180 NFUs). These results could be related to a higher nitrogen agronomic efficiency in the combined fertilisation treatments that do not exceed the total NFUs required by the crop. Combined fertilisation was also an effective fertiliser technique to store total nitrogen and organic carbon in the soil. However, compared to the reference mineral fertilisation (180 NFUs), no significant changes in the soil organic carbon were observed, probably due to the crop management method in which the straw is removed and to higher gas emissions. Our results support the need to assess the efficacy of each agricultural technique at local scales in order not to overestimate or underestimate the potential of each agricultural technique to store soil organic carbon.