We present a pulsed laser deposition (PLD) system that can monitor growth by simultaneously using in situ optical spectroscopic ellipsometry (SE) and reflection highenergy electron diffraction (RHEED). The RHEED precisely monitors the number of thin-film layers and surface structure during the deposition and the SE measures the optical spectra of the samples simultaneously. The thin-film thickness information obtained from RHEED facilitates the SE modeling process, which allows extracting the in situ optical spectra, i.e. the dielectric functions, of thin-films during growth. The in situ dielectric functions contain indispensable information about the electronic structure of thin-films. We demonstrate the performance of this system by growing LaMnO 3+δ (LMO) thin-films on SrTiO 3 (001) substrates. By using in situ SE and RHEED simultaneously, we show that real-time thickness and dielectric functions of the LMO thin-films can be effectively extracted. The simultaneous monitoring of both optical SE and RHEED offers important clues to understand the growth mechanism of atomic-scale thin-films. a)