AbstractQuantum chemistry (QC) is one of the most promising applications of quantum computing. However, present quantum processing units (QPUs) are still subject to large errors. Therefore, noisy intermediate‐scale quantum (NISQ) hardware is limited in terms of qubit counts/circuit depths. Variational quantum eigensolver (VQE) algorithms can potentially overcome such issues. Here, we introduce the OpenVQE open‐source QC package. It provides tools for using and developing chemically‐inspired adaptive methods derived from unitary coupled cluster (UCC). It facilitates the development and testing of VQE algorithms and is able to use the Atos Quantum Learning Machine (QLM), a general quantum programming framework enabling to write/optimize/simulate quantum computing programs. We present a specific, freely available QLM open‐source module, myQLM‐fermion. We review its key tools for facilitating QC computations (fermionic second quantization, fermion‐spin transforms, etc.). OpenVQE largely extends the QLM's QC capabilities by providing: (i) the functions to generate the different types of excitations beyond the commonly used UCCSD ansatz; (ii) a new Python implementation of the “adaptive derivative assembled pseudo‐Trotter method” (ADAPT‐VQE). Interoperability with other major quantum programming frameworks is ensured thanks to the myQLM‐interop package, which allows users to build their own code and easily execute it on existing QPUs. The combined OpenVQE/myQLM‐fermion libraries facilitate the implementation, testing and development of variational quantum algorithms, while offering access to large molecules as the noiseless Schrödinger‐style dense simulator can reach up to 41 qubits for any circuit. Extensive benchmarks are provided for molecules associated to qubit counts ranging from 4 to 24. We focus on reaching chemical accuracy, reducing the number of circuit gates and optimizing parameters and operators between “fixed‐length” UCC and ADAPT‐VQE ansätze.This article is categorized under: Software > Quantum Chemistry Quantum Computing > Algorithms