Recently, a proper genuine multipartite entanglement measure has been found for three-qubit pure states [see Xie and Eberly, Phys. Rev. Lett. 127, 040403 (2021)PRLTAO0031-900710.1103/PhysRevLett.127.040403], but capturing useful entanglement measures for mixed states has remained an open challenge. So far, it requires not only a full tomography in experiments, but also huge calculational labor. A leading proposal was made by Gühne, Reimpell, and Werner [Phys. Rev. Lett. 98, 110502 (2007)PRLTAO0031-900710.1103/PhysRevLett.98.110502], who used expectation values of entanglement witnesses to describe a lower bound estimation of entanglement. We provide here an extension that also gives genuine upper bounds of entanglement. This advance requires only the expectation value of any Hermitian operator. Moreover, we identify a class of operators A_{1} that not only give good estimates, but also require a remarkably small number of experimental measurements. In this Letter, we define our approach and illustrate it by estimating entanglement measures for a number of pure and mixed states prepared in our recent experiments.