Thermally integrated Carnot battery (TICB) emerges as a promising technology for long-duration energy storage. This study aims to improve its multi-dimensional performance from the optimization design level, thereby promoting its competitiveness. Firstly, a refined system architecture is developed, integrating subsystem layout modification and advanced thermal integration mode. Sixteen potential working fluid pairs are formed by screening low-GWP refrigerants as drop-in substitutes for R245fa. Then, a comprehensive evaluation framework is established to characterize this technology from energy, exergy, and economic perspectives, and a collaborative optimization method is introduced to facilitate integrated optimization. Finally, a whole cycle cumulative exergy analysis is conducted to explore directions for further improvement. Results indicate that, compared to the basic architecture, the round-trip efficiency (RTE) of the proposed system is elevated by over 30%. The use of different alternative refrigerants in the charging and discharging cycles makes the TICB not only sustainable but also more efficient. The thermodynamic dilemma of determining the heat pump evaporation temperature disappears with a closed-type heat source. To maximize overall thermo-economics, sufficient heat pump subcooling and evaporator internal superheat are necessary, and the ideal storage temperature span and pinch point temperature difference of heat exchangers must be identified. The collaborative optimization displays that the first-rank working fluid pair is R1234ze(Z)-R1224yd(Z), with an RTE of 85.2%, a volumetric energy density of 3.10 kWh/m3, and a levelized cost of storage of 0.303 $/kWh, respectively. Furthermore, the RTE is highly sensitive to the insulation quality of storage tanks. A mere 2.5% performance degradation can lead to a 10% points decline in RTE. Internal exergy destruction is primarily caused by poor heat transfer matching, while external exergy loss mainly results from underutilized heat sources during non-charging periods. Therefore, we recommend the district heating network as the target heat source for the dual-period TICB. These achievements offer a valuable reference for the research and development of efficient, affordable, and sustainable TICB.