Owing to its light weight and corrosion resistance, the concrete-filled fiber-reinforced polymer tube (CFFT) structure has a broad application prospect; the concrete compactness is key to the strength of CFFTs. To meet the urgent requirement of compactness monitoring of CFFTs, a quantitative method, which uses an array of four equally spaced piezoceramic patches and an ultrasonic time difference of arrival (TDOA) algorithm, is developed. Since the velocity of the ultrasonic wave propagation in fiber-reinforced polymer (FRP) material is about half of that in concrete material, the compactness condition of CFFT impacts the piezoceramic-induced wave propagation in the CFFT, and differentiates the TDOA for different receivers. An important condition is the half compactness, which can be judged by the Half Compactness Indicator (HCI) based on the TDOAs. To characterize the difference of stress wave propagation durations from the emitter to different receivers, which can be utilized to calculate the concrete infill compactness, the TDOA ratio (TDOAR) is introduced. An innovative algorithm is developed in this paper to estimate the compactness of the CFFT using HCI and TDOAR values. Analytical, numerical, and experimental studies based on a CFFT with seven different states of compactness (empty, 1/10, 1/3, 1/2, 2/3, 9/10, and full) are carried out in this research. Analyses demonstrate that there is a good agreement among the analytical, numerical, and experimental results of the proposed method, which employs a piezoceramic transducer array and the TDOAR for quantitative estimating the compactness of concrete infill in a CFFT.