This paper proposes an active radio frequency (RF) cancellation solution to suppress the transmitter (TX) passband leakage signal in radio transceivers supporting simultaneous transmission and reception. The proposed technique is based on creating an opposite-phase baseband equivalent replica of the TX leakage signal in the transceiver digital front-end through adaptive nonlinear filtering of the known transmit data, to facilitate highly accurate cancellation under a nonlinear TX power amplifier (PA). The active RF cancellation is then accomplished by employing an auxiliary transmitter chain, to generate the actual RF cancellation signal, and combining it with the received signal at the receiver (RX) low noise amplifier (LNA) input. A closed-loop parameter learning approach, based on the decorrelation principle, is also developed to efficiently estimate the coefficients of the nonlinear cancellation filter in the presence of a nonlinear TX PA with memory, finite passive isolation, and a nonlinear RX LNA. The performance of the proposed cancellation technique is evaluated through comprehensive RF measurements adopting commercial LTE-Advanced transceiver hardware components. The results show that the proposed technique can provide an additional suppression of up to 54 dB for the TX passband leakage signal at the RX LNA input, even at considerably high transmit power levels and with wide transmission bandwidths. Such novel cancellation solution can therefore substantially improve the TX-RX isolation, hence reducing the requirements on passive isolation and RF component linearity, as well as increasing the efficiency and flexibility of the RF spectrum use in the emerging 5G radio networks.