Beams of protons were smashed into each other Thursday at four observation positions with collision energies of 8 trillion electron volts, a world record, the BBC reported.
The increase in energy significantly improves the collider's ability to make discoveries in so-called new physics, researchers said.
"The experience of two good years of running at 3.5 TeV per beam gave us the confidence to increase the energy for this year without any significant risk to the machine," Steve Myers, the director for accelerators and technology at CERN, said. "Now it's over to the experiments to make the best of the increased discovery potential we're delivering them!"
Since its first operations in 2008, LHC operators have incrementally increased the energy contained in each of the beams of protons sent around the 16-mile collider, which lies beneath the Franco-Swiss border.
The ultimate goal, researchers said, is an operating proton beam energy of 14 trillion electron volts.
"The increase in energy is all about maximizing the discovery potential of the LHC," said CERN Research Director Sergio Bertolucci. "And in that respect, 2012 looks set to be a vintage year for particle physics."