Controllable synthesis of Metal‐organic frameworks (MOFs) with well‐defined morphology, composition and size is of great importance towards understanding their structure‐property relationship in various applications. Herein, the effect of morphology of photocatalysts on their optical behavior and photocatalytic efficiency was identified utilizing physical synthetic parameters for methylene blue removal. For this purpose, MIL‐53(Fe) was fabricated as an efficient photocatalyst via solvothermal approach using chloride and nitrate salts as different secondary block unit (SBU) sources. Each of the powders obtained by two metal sources was synthesized at three different temperatures (120, 150, and 180 °C). The fabricated MOFs were methodically investigated and characterized in terms of structural, textural, morphological and optical. The obtained empirical data confirmed that the particles synthesized at 120 °C using iron chloride exhibit the highest efficiency for methylene blue removal. This could be associated to their high surface area and UV light absorption in comparison with other samples. These results can be considered in future research to maximize degradation of organic dyes as a serious pollutant in wastewater.