A Google spokesperson said: "We comply with the tax law in Spain, as in every other country in which we operate. We are cooperating fully with the authorities in Madrid to answer their questions, as always."
Today's police search comes a little over a month after police raided the technology giant's French headquarters on tax evasion suspicions.
In a statement, the French prosecutors office revealed that the purpose of the raid was to discover whether Google Ireland had a permanent base in France and, if so, whether the company was failing in its fiscal duty to report activities that should be taxed in France.
Google has recently come under fire over its tax position, with a so-called sweetheart deal with HM Revenue & Customs (HMRC) for £130m in unpaid corporation tax sparking the public's interest in particular.
In a hearing by the Public Accounts Committee (PAC), representatives from the technology giant found themselves having to defend their company's activities in tax havens, which the MPs claimed the organisation had no real purpose of operating in other than to take advantage of tax loopholes with names such as "double Irish Dutch sandwich".
Earlier this week, the PAC revealed an open letter signed by the chairs of parliamentary finance committees of Germany, Hungary, Finland, Norway and Slovakia, along with senior MPs from the Netherlands, Czech Republic and Bulgaria, which urged their respective governments to introduce measures to promote tax transparency from multinational companies.