Real-time acquisition of the morphological information of nanomaterials is crucial to achieving morphological controllable synthesis, albeit being challenging. A novel device was designed, which integrated dielectric barrier discharge (DBD) plasma synthesis and simultaneous in situ spectral monitoring of the formation of metal-organic frameworks (MOFs). Important dynamic luminescence behaviors such as coordination induced emission (CIE), antenna effect (AE), and red-blue shift were continuously captured to reveal the spectral emission mechanism and energy transfer progress and verify the correlation with the morphological evolution of the MOFs. The prediction and control of morphology were successfully achieved with Eu(TCPP) as a model MOF. The proposed method will shed new light on exploring the spectral emission mechanism, energy conversion and in situ morphology monitoring of other luminescent materials.