The proportion of people living in social exclusion stood at 25.1 percent in mid-2013, up from 16.3 percent in 2007, a year before a decade-long housing bubble collapsed sending the economy into a tailspin, Caritas said in a massive 700-page report.
Of the 11.7 million people who live in social exclusion, 77.1 percent do not have a job and 61.7 percent struggle to keep a roof over their heads.
"Without getting into the economic debate over whether we are in a new growth cycle or not, we must note there are no signs that the tendency towards worsening social problems has not stopped," the report said.
Spain has shown a gradual economic pick-up since emerging from recession in mid-2013, and clocked up growth of 0.6 percent in the second quarter of 2014 — the fastest growth in six years — but still suffers from a 23.7-percent unemployment rate, one of the highest in the industrialized world.
The government forecasts the economy will grow 1.3 percent in 2014, bouncing back after six years of crisis that brought it close to financial collapse.
"Economic growth on its own does not lead to equality," Caritas secretary general Sebastian Mora told a news conference.
"What is clear is that to fight poverty and social exclusion, you need to boost social protection. It is true that there have been programmes and plans....but these efforts are absolutely insufficient."
Prime Minister Mariano Rajoy's conservative government has implemented the steepest spending cuts since Spain returned to democracy in the mid-1970s in order to rein in a ballooning public deficit.
Some half a million Spanish households have no source of income, according to Caritas.
The charity said the economic downturn has hit immigrants, especially those from outside the European Union, especially hard.
More than half of all foreigners from outside the European Union, 52.6 percent, lived in social exclusion in mid-2013 compared with 20.6 percent of all Spaniards.
Tuesday also saw the release of a Unicef report into childhood poverty which showed that Spanish households lost a decade's worth of progress from 2008 to 2012 in terms of median income.
The proportion of Spanish children living in poverty rose from 28.2 percent to 36.3 percent in the same period, the Unicef study found, while the number of 15 to 24-year-olds who were neither studying nor working climbed from 14.3 percent to 18.6 percent.