At loggerheads with the separatist government in the northeastern region, which plans to hold a Scotland-style independence referendum against Madrid's will, Rajoy has launched a so-called "operation dialogue" in a bid to ease tensions and win over public opinion.
Criticised for inaction during his first term in office as independence fervour mounted in Catalonia, Rajoy promised to strive for a rapprochement when he took power again in November to solve what he has dubbed Spain's most serious problem.
Lack of investment in the wealthy but indebted region has long been a source of contention, pushing some weary Catalans to come out in support of independence, particularly as they see their tax money sent to Madrid and used to prop up other poorer regions.
The belated arrival of the high-speed train to Barcelona in 2008, 16 years after the first such link to Seville in the south, a lack of free highways, and delays in commuter trains are just some of the issues that have contributed to this weariness.
Hoping to lure them back, Rajoy pledged to pour money into the commuter train network, airports, roads and ports.
He also promised to finish by 2020 the Catalan section of a Mediterranean freight railway link due to go through coastal regions all the way down to Algeciras on Spain's southern tip.
In addition, Rajoy said he would address the long-time complaint about regional funding and taxes.
"This matters to me. I want Catalonia to be prosperous in a thriving Spain," he said, asking companies for "help in winning the battle for moderation".
"Promises of investment in Catalonia made by the Spanish government have lost all credibility in the eyes of Catalan society," Puigdemont said in an article penned with his deputy Oriol Junqueras and published today in the regional daily El Periodico.
They said the central government's previous investment pledges had only been partially fulfilled.
"The state's investment in Catalonia represents 8.2 percent of total investment in regions," they said, arguing this was "way below" what it should be getting given the wealth it generates and how populous it is.
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