Theoretically understanding and experimentally characterizing and modifying the underlying Hamiltonian of a quantum system is of utmost importance in achieving high-fidelity quantum gates for quantum computing. In this work, we explore the use of dynamical decoupling (DD) in characterizing undesired two-qubit couplings as well as the underlying single-qubit decoherence, and in suppressing them. We develop a syncopated dynamical decoupling technique which protects against decoherence and selectively targets unwanted two-qubit interactions, overcoming both significant hurdles to achieving precise quantum control and realizing quantum computing on many hardware prototypes. On a transmon-qubit-based superconducting quantum device, we identify separate white and $1/f$ noise components underlying the single-qubit decoherence and a static ZZ coupling between pairs of qubits. We suppress these errors using syncopated dynamical decoupling in two-qubit benchmarking experiments and significantly boost performance in a realistic algorithmic quantum circuit.
