With 10 systems purchased every second worldwide, the University of NSW professor fears the cooling technology has become the default response to rising global temperatures.
"We cannot air-condition our way out of climate change," he said.
"If every building depends entirely on mechanical cooling, we create enormous pressure on electricity systems while adding even more heat to our cities."
Days of 40C in usually temperate European cities has brought urban heat into focus, with more frequent and severe heatwaves linked to growing atmospheric concentrations of greenhouse gases.
In Australia, an El Nino on top of global temperature rise could lead to challenging summer conditions, particularly in heatwave hotspots such as western Sydney.
Cities swelter through higher temperatures worse than surrounding farm and bushland as man-made materials such as asphalt and concrete absorb rather than reflect sun radiation.
Prof Santamouris says cities can benefit from passive cooling strategies that stop heat entering buildings, such as ventilation and sunlight-reflecting roofs, according to a global review from the academic and RMIT's Konstantina Vasilakopoulou.
For example, research suggests widespread use of "cool roofs" - which reflect solar energy through design, colour and material choice - could lower ambient urban temperatures by about 1-2C.
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