The increasing significance of theorem proving-based formalization in mathematics and computer science highlights the necessity for formalizing foundational mathematical theories. In this work, we employ the Coq interactive theorem prover to methodically formalize the language, semantics, and syntax of propositional logic, a fundamental aspect of mathematical reasoning and proof construction. We construct four Hilbert-style axiom systems and a natural deduction system for propositional logic, and establish their equivalences through meticulous proofs. Moreover, we provide formal proofs for essential meta-theorems in propositional logic, including the Deduction Theorem, Soundness Theorem, Completeness Theorem, and Compactness Theorem. Importantly, we present an exhaustive formal proof of the Completeness Theorem in this paper. To bolster the proof of the Completeness Theorem, we also formalize concepts related to mappings and countability, and deliver a formal proof of the Cantor–Bernstein–Schröder theorem. Additionally, we devise automated Coq tactics explicitly designed for the propositional logic inference system delineated in this study, enabling the automatic verification of all tautologies, all internal theorems, and the majority of syntactic and semantic inferences within the system. This research contributes a versatile and reusable Coq library for propositional logic, presenting a solid foundation for numerous applications in mathematics, such as the accurate expression and verification of properties in software programs and digital circuits. This work holds particular importance in the domains of mathematical formalization, verification of software and hardware security, and in enhancing comprehension of the principles of logical reasoning.