The group is spending $50,000 on a week of ads attacking Sens. Mark Pryor (Ark.), Mark Begich (Alaska), Mary Landrieu (La.) and Kay Hagan (N.C.) on the issue, all vulnerable red-state Democrats who've come under fire from Crossroads before.
"While even President Obama and the majority of House Members agree on a long-term bipartisan plan to give America's college students relief on their student loans, Sen. Begich voted to put partisan posturing ahead of getting a broadly supported deal done," the ad reads.
It charges that the senator "is holding your future hostage," and that they "broke with moderate Senate colleagues" to help block reform.
"Instead of acting to provide a practical solution to student loan rates, Sen. Begich voted to leave students at the mercy of crass Washington gamesmanship," the ad continues, and urges viewers to call their senator.
Though the Republican-controlled House passed a measure to prevent current student loan rates from doubling on July 1, the Senate was unable to follow suit as their work on immigration reform consumed much of their time before the July 4 recess.
A Democratic-backed fix failed in the upper chamber on Wednesday, unable to gain any Republican support. Senate Republicans are backing a measure sponsored by Sens. Angus King (I-Maine) and Joe Manchin (D-W.Va.) that's similar to the House-passed legislation, but Senate Democrats remain largely opposed to the bill.
Crossroads GPS Communications Director Jonathan Collegio suggested the blame lies on the shoulders not just of Democratic senators who remain opposed to the House bill, but of Senate Majority Leader Harry Reid (D-Nev.).
"The message here is that not only did Senators Pryor, Begich, Landrieu and Hagan screw up by effectively supporting a massive rate hike on college students, but Harry Reid screwed up by making his members walk the plank on incredibly amateur strategy," he said.
"Harry Reid exposed his caucus to the wrath not only of college students, but of local editorial pages and citizens who value common sense above all. The Senate needs to pass the House plan without delay."
The hike in loan rates has been used as a political bludgeon by both sides in recent weeks, with Democrats charging that the Republican fix would ultimately result in higher loan rates for students.
The potential political fallout of rising rate hikes helped Congress pass a fix last year, amidst a presidential race and urging from both Obama and Republican presidential nominee Mitt Romney, but the path forward this year remains murky.