Engineered cementitious composites (ECCs) are special types of fibre-reinforced cementitious composites (FRCC) with higher strain capacity which can be achieved with low fibre volume as low as 2% and total elimination of coarse aggregates. Due to the outstanding performance of ECCs, they are suitable for various construction and repair applications. However, in order for ECCs to achieve their properties; a high amount of binder which is primarily composed of Portland cement (PC) is used alongside a special type of ultrafine silica sand (USS) which is different from the conventional natural fine aggregates. The production of PC is known to be detrimental to the environment due to its high carbon dioxide emissions coupled with the high consumption of natural resources. Thus, the high use of PC content in ECCs posed a sustainability threat. Similarly, the USS used in ECCs are not readily available everywhere and are expensive. The processing of the USS coupled with its transportation over long distances would also increase the cost and embodied carbon of ECCs. Hence, in order to promote more development and applications of ECCs for various applications; this dissertation aims to provide innovative ways to improve the sustainability of ECCs and their performances. This dissertation offers four solutions to improve the sustainability of ECCs which are (i) use of unconventional industrial by-products as partial replacement of PC (ii) total replacement of PC in ECCs with alternative sustainable binders (iii) replacement of USS in ECCs with recycled materials and (iv) the use of supplementary cementitious materials to replace a high volume of PC. The findings from this study revealed sustainable ECCs with acceptable mechanical and durability performance can be achieved with the use of alternative binders or replacement of the conventional USS used in ECC mixtures. The sustainability and cost assessment of the ECCs indicated that the incorporation of industrial by-products such as blast furnace slag (BFS) especially at higher content is beneficial to reducing the negative environmental impact and economic burden associated with ECCs compared to the conventional ECC. The sustainability index and cost index of the ECCs further showed that the use of BFS is more beneficial when the sustainability and cost of the ECCs are compared with the corresponding performance. Similarly, the use of recycled materials as an alternative to USS was found to result in a significant reduction in the embodied carbon and cost of ECCs. The use of recycled materials such as expanded glass (EG) as aggregates in ECCs was also found to improve the thermal insulation properties of ECCs making such ECC suitable for the production of building envelope elements.