Bio-based materials are gaining attention across various industrial sectors as sustainable alternative to conventional materials, with a significant emphasis on concrete – the most widely used construction material. The incorporation of natural fibres provides technical, environmental, and economic advantages. Derived from renewable resources, these fibres reduce carbon footprint, and provide non-toxicity, biodegradability, corrosion resistance, and wide availability. However, they typically possess lower strength, and reduced durability compared to synthetic fibres. Presented study aims to compare not only the mechanical properties of selected natural and synthetic fibres but also their environmental impact. Natural fibres flax, hemp, jute, and sisal in the form of yarn, and synthetic rovings alkali-resistant glass, basalt and carbon were fabricated into continuous fibre composite reinforcement (CFCR). Their tensile strength was evaluated, and they were utilized as reinforcement of thin high-performance concrete (HPC) plates tested in a four-point bending test. The flax and hemp yarn CFCRs showed as viable reinforcement of HPC structures, while carbon-hemp hybrid showed great potential due to its good mechanical performance and less brittle behaviour. The following LCA analysis was performed in compliance with EN 15804:2012 + A2:2019/AC:2021. The results showed that natural fibres significantly reduced the carbon footprint of the concrete samples. However, the incorporation of natural fibres in concrete slabs increased the environmental impact across several categories, particularly acidification, and eutrophication, primarily due to the use of pesticides, herbicides, and fertilizers.