AlmostEquals(ref a, ref b).Should().BeTrue("because matrices a and b are almost equal");
AlmostEquals(ref a, ref b, epsilon).Should().BeTrue("because matrices a and b are almost equal");
You can even add some info about the matrices and epsilon into the message like
AlmostEquals(ref a, ref b, epsilon).Should().BeTrue("because matrices a and b are almost equal with {0} precision", epsilon);
May be you would need to introduce a local bool variable to make the FluentAssertions work (I don't have it installed) and assign it a value of AlmostEquals and then run assertion against the boolean variable.