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Superior carbon fixation rate of microalgae compared to terrestrial biomass offers a significant opportunity to build a reliable carbon supply chain for carbon source. Extremophilic microalgae, Galdieria sulphuraria (G. sulphuraria), is further underscored by its exceptional adaptability to harsh environments such as wastewater. This study proposed a strategy to efficiently utilize carbon in G. sulphuraria and to valorise metallic industrial waste, particularly red mud (RM), through co-pyrolysis. To improve the eco-friendliness, CO 2 was used as a reactive gas medium in pyrolysis system. Use of CO 2 in single-stage pyrolysis of G. sulphuraria leads to the enhanced formation of CO through gas-phase reactions (GPRs) of it with volatile matter (VM). Specifically, CO 2 partially oxidize VM while reduce into CO. From single-stage co-pyrolysis of G. sulphuraria with RM, RM accelerated the reaction kinetics for GPRs between CO 2 and VM, leading to the increased formation of syngas from 27.5 to 37.6 mmol compared to N 2 environment. From multi-stage co-pyrolysis, an additional heat source (700 °C) facilitated the GPRs induced by CO 2 , increasing evolution syngas from 37.6 to 73.8 mmol compared to single-stage co-pyrolysis under CO 2 environment. RM‑carbon composites (RMCs) from co-pyrolysis of G. sulphuraria with RM under N 2 /CO 2 environments was utilized as a catalyst in thermally induced transesterification. Both RMCs exhibited superior performance over commercial silica. In specific, both RMCs resulted in higher biodiesel yields of >95.0 wt% at 300 °C, compared to commercial silica (biodiesel yield of 16.6 wt% at corresponding reaction temperature). Such performance of RMCs in thermally induced transesterification could be improved by the modification of their surface properties but its related study was not conducted in this stage. A series of experimental findings propose that co-pyrolysis of G. sulphuraria and RM creates opportunities to maximise syngas production and fabricate red mud‑carbon composites to enhance biodiesel conversion efficiency. [Display omitted] • Tolerance to harsh conditions makes Galdieria sulphuraria a reliable carbon source. • Co-pyrolysis of microalgae and red mud waste produces iron-carbon composite. • CO 2 -assisted pyrolysis improves CO formation, promoting syngas production. • Iron-carbon composite catalyzes in thermally induced transesterification reaction. [ABSTRACT FROM AUTHOR]

• Algal-biomass-derived (R)-GVL production with perfect enantiomeric excess (>99.99) • LA was obtained from G. verrucosa through acidic hydrothermal conversion. • Chemoenzymatic reaction converted LA to (R)-GVL via 4-HV. • Residual algal biomass was used to prepare anode for LiB via simple heat treatment. • The results can construct to viable zero-waste biorefinery and circular bioeconomy. Mankind is facing a severe climate crisis caused by fossil fuel-derived CO 2 emissions. Although biorefineries utilizing biomass have been considered the best option for carbon-neutrality, most biorefinery-derived products have not yet been promising for economic feasibility; various strategies have been developed to increase economic competitiveness, and zero-waste biorefineries are challenging options. Herein, we aim to develop an algal biomass-based zero-waste biorefinery for producing enantioselective (R)-γ-valerolactone ((R)-GVL) and carbonaceous electrodes applicable for Li-ion batteries (LiBs). Various algal biomasses were hydrothermally oxidized to produce levulinic acid (LA) as an intermediate for producing (R)-GVL, resulting that Gracilaria verrucosa was selected as feedstock. For the hydroxylation of G. verrucosa -derived LA to 4-hydroxyvaleric acid (4-HV), 3-hydroxybutyrate dehydrogenase (HBDH) was explored through genome mining and further engineered. The engineered HBDH successfully converted G. verrucosa -derived LA to 4-HV, which was subsequently lactonized under acidic conditions, resulting in optically pure (R)-GVL. To our knowledge, this is the first report of the production of an algal biomass-derived enantioselective (R)-GVL with a perfect enantiomeric excess (>99.99 %) that can be used as a precursor for more valuable biopharmaceuticals and bioplastics than biofuels. Furthermore, residual G. verrucosa after hydrothermal oxidation was used as a carbonaceous anode material for LIBs for the first time; hard carbon anodes, which were prepared through simple heat treatment (800 ℃, 3 h, argon atmosphere), exhibit good capacities of 231, 191, 133, 108, 97 and 86 mAh/g at 0.05, 0.1, 0.5, 1, 1.5, and 2 A/g, respectively. The results discussed herein can provide insights into zero-waste biorefineries applicable for diverse industrial fields (e.g., biopolymer, biopharmaceutical and energy storage) and contribute to the construction of closed-carbon-loops for coping with climate change. [ABSTRACT FROM AUTHOR]