Three zinc(II) metal-organic frameworks, [Zn2(oba)2(4-bpdb)]·(TMU-4), [Zn(oba)(4-bpdh)0.5]n·(TMU-5) and [Zn(oba)(4-bpmb)0.5]n·(TMU-6), (H2oba = 4,4'-oxybisbenzoic acid, 4-bpdb = 1,4-bis(4-pyridyl)-2,3-diaza-1,3-butadiene, 4-bpdh = 2,5-bis(4-pyridyl)-3,4-diaza-2,4-hexadiene and 4-bpmb = N1,N4-bis((pyridin-4-yl)methylene)benzene-1,4-diamine), containing azine-functionalized pores have successfully been synthesized via mechanosynthesis as a convenient, rapid, solventless and green process. These MOFs were studied for degradation of congo red from aqueous solutions under UV and/or visible light irradiation without auxiliary oxidants such as H2O2. TMU-6 could decolorize 100 ppm of congo red readily and quickly within 90 min, exhibiting about 68.4% in COD reduction after 72 h of UV irradiation. These results suggest that TMU-6/UV photocatalysis may be envisaged as a method for treatment of diluted colored waste waters not only for decolorization, but also for detoxification in textile industries.